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Embedding oxophilic rare-earth single atom in platinum nanoclusters for efficient hydrogen electro-oxidation.

ABSTRACT: Designing Pt-based electrocatalysts with high catalytic activity and CO tolerance is challenging but extremely desirable for alkaline hydrogen oxidation reaction. Herein we report the design of a series of single-atom lanthanide (La, Ce, Pr, Nd, and Lu)-embedded ultrasmall Pt nanoclusters for efficient alkaline hydrogen electro-oxidation catalysis based on vapor filling and spatially confined reduction/growth of metal species. Mechanism studies reveal that oxophilic single-atom lanthanide species in Pt nanoclusters can serve as the Lewis acid site for selective OH^- adsorption and regulate the binding strength of intermediates on Pt sites, which promotes the kinetics of hydrogen oxidation and CO oxidation by accelerating the combination of OH^- and *H/*CO in kinetics and thermodynamics, endowing the electrocatalyst with up to 14.3-times higher mass activity than commercial Pt/C and enhanced CO tolerance. This work may shed light on the design of metal nanocluster-based electrocatalysts for energy conversion.

SUBMITTER: Wang X

PROVIDER: S-EPMC10290706 | biostudies-literature | 2023 Jun

REPOSITORIES: biostudies-literature

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Embedding oxophilic rare-earth single atom in platinum nanoclusters for efficient hydrogen electro-oxidation.

Wang Xiaoning X Tong Yanfu Y Feng Wenting W Liu Pengyun P Li Xuejin X Cui Yongpeng Y Cai Tonghui T Zhao Lianming L Xue Qingzhong Q Yan Zifeng Z Yuan Xun X Xing Wei W

Nature communications 20230624 1

Designing Pt-based electrocatalysts with high catalytic activity and CO tolerance is challenging but extremely desirable for alkaline hydrogen oxidation reaction. Herein we report the design of a series of single-atom lanthanide (La, Ce, Pr, Nd, and Lu)-embedded ultrasmall Pt nanoclusters for efficient alkaline hydrogen electro-oxidation catalysis based on vapor filling and spatially confined reduction/growth of metal species. Mechanism studies reveal that oxophilic single-atom lanthanide specie ...[more]

PMID: 37355646

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Project description:The Moon-forming giant impact extensively melts and partially vaporizes the silicate Earth and delivers a substantial mass of metal to Earth's core. The subsequent evolution of the magma ocean and overlying atmosphere has been described by theoretical models but observable constraints on this epoch have proved elusive. Here, we report thermodynamic and climate calculations of the primordial atmosphere during the magma ocean and water ocean epochs respectively and forge new links with observations to gain insight into the behavior of volatiles on the Hadean Earth. As accretion wanes, Earth's magma ocean crystallizes, outgassing the bulk of its volatiles into the primordial atmosphere. The redox state of the magma ocean controls both the chemical composition of the outgassed volatiles and the hydrogen isotopic composition of water oceans that remain after hydrogen escape from the primordial atmosphere. The climate modeling indicates that multi-bar H2-rich atmospheres generate sufficient greenhouse warming and rapid kinetics resulting in ocean-atmosphere H2O-H2 isotopic equilibration. Whereas water condenses and is mostly retained, molecular hydrogen does not condense and can escape, allowing large quantities (~102 bars) of hydrogen - if present - to be lost from the Earth in this epoch. Because the escaping inventory of H can be comparable to the hydrogen inventory in primordial water oceans, equilibrium deuterium enrichment can be large with a magnitude that depends on the initial atmospheric H2 inventory. Under equilibrium partitioning, the water molecule concentrates deuterium and, to the extent that hydrogen in other forms (e.g., H2) are significant species in the outgassed atmosphere, pronounced D/H enrichments (~1.5-2x) in the oceans are expected from equilibrium partitioning in this epoch. By contrast, the common view that terrestrial water has a carbonaceous chondritic source requires the oceans to preserve the isotopic composition of that source, undergoing minimal D-enrichment via equilibration with H2 followed by hydrodynamic escape. Such minimal enrichment places upper limits on the amount of primordial atmospheric H2 in contact with Hadean water oceans and implies oxidizing conditions (logfO2>IW+1, H2/H2O<0.3) for outgassing from the magma ocean. Preservation of an approximate carbonaceous chondrite D/H signature in the oceans thus provides evidence that the observed oxidation of silicate Earth occurred before crystallization of the final magma ocean, yielding a new constraint on the timing of this critical event in Earth history. The seawater-carbonaceous chondrite "match" in D/H (to ~10-20%) further constrains the prior existence of an atmospheric H2 inventory - of any origin - on post-giant-impact Earth to <20 bars, and suggests that the terrestrial mantle supplied the oxidant for the chemical resorption of metals during terrestrial late accretion.

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Embedding oxophilic rare-earth single atom in platinum nanoclusters for efficient hydrogen electro-oxidation.

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Embedding oxophilic rare-earth single atom in platinum nanoclusters for efficient hydrogen electro-oxidation.

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